highlight 9 2019

Using a combination of ultrafast spectroscopy, molecular dynamics (MD) simulations, and quantum calculations, we have recently demonstrated that ion pairs generated by CT excitation of an electron donor/acceptor (DA) complex exhibit rich structural dynamics (PCCP 2019, 21, 11797). These dynamics are expected to modulate the electronic coupling matrix element, and consequently the charge recombination rate, due to the its sensitivity to DA orientation and separation. Generalized Mulliken-Hush calculations on representative MD generated benzene/tetracyanoethylene pairs demonstrate that the structural heterogeneity and dynamics of the pairs induce broad distributions (Figure A) and large fluctuations (Figure B) in the electronic coupling. Future modeling of charge recombination in these pairs must take these fluctuations into account, as the pair cannot be considered a single, static, species.

Select Highlight





Eric Vauthey

Physical Chemistry Department - Sciences II - University of Geneva
30, Quai Ernest Ansermet - CH-1211 Geneva 4 (Switzerland)

© All rights reserved by Eric Vauthey and the University of Geneva

Design and code by Guillaume Duvanel